Dynamics of heavy metal accumulation in thalli of the epiphytic lichen Hypogymnia physodes

A sequential extraction procedure was used to study localization of heavy metals in thalli of the lichen Hypogymnia physodes (L.) Nyl. growing under conditions of chronic aerotechnogenic pollution in the Middle Urals. Trends in the seasonal dynamics of metal contents in the thalli were revealed. The dynamics of metal accumulation was also studied in the thalli brought to the polluted zone from the background environment. After one year, the extra-and intercellular contents of most metals in these transplants approached those in the aboriginal thalli and in some cases (intracellular content of cadmium) exceeded them.     

On monitoring anthropogenic airborne uranium concentrations and (235)U/(238)U isotopic ratio by Lichen - bio-indicator technique

Lichens are widely used to assess the atmospheric pollution by heavy metals and radionuclides. However, few studies are available in publications on using lichens to qualitatively assess the atmospheric pollution levels. The paper presents research results applying epiphytic lichens as bio-monitors of quantitative atmospheric contamination with uranium. The observations were conducted during 2.5 years in the natural environment. Two experimental sites were used: one in the vicinity of a uranium contamination source, the other one - at a sufficient distance away to represent the background conditions. Air and lichens were sampled at both sites monthly. Epiphytic lichens Hypogimnia physodes were used as bio-indicators. Lichen samples were taken from various trees at about 1.5m from the ground. Air was sampled with filters at sampling stations. The uranium content in lichen and air samples as well as isotopic mass ratios (235)U/(238)U were measured by mass-spectrometer technique after uranium pre-extraction. Measured content of uranium were 1.45 mgkg(-1) in lichen at 2.09 E-04 microgm(-3) in air and 0.106 mgkg(-1) in lichen at 1.13 E-05 microgm(-3) in air. The relationship of the uranium content in atmosphere and that in lichens was determined, C(AIR)=exp(1.1 x C(LICHEN)-12). The possibility of separate identification of natural and man-made uranium in lichens was demonstrated in principle.     

Stable nitrogen isotopes (δ15N) in thalli of the lichen Hypogymnia physodes along a altitudinal gradient in the Khangai Plateau, Mongolia

Stable nitrogen isotopes (??¹⁵N) have been determined in the organic matter (OM) of thalli of the lichen Hypogymnia physodes (L.) Nyl. collected at 15 levels along an altitudinal gradient (1250?C2928 m a.s.l.) in forest and alpine meadow communities of the Khangai Plateau, Mongolia. The results show that, in the study region as a whole, no correlation between the ??¹⁵N content and elevation is observed. However, the lichen OM within the mountain forest belt is depleted of the heavy ¹⁵N isotope as elevation increases (from 1250 to 2400 m a.s.l.), whereas in the alpine meadow belt (2500?C2928 m a.s.l) it is enriched with this isotope. In addition, ??¹⁵N values in OM show an inverse dependence on the relative content of total nitrogen in the thalli.     

Radioisotope contaminations from releases of the Tomsk-Seversk nuclear facility (Siberia, Russia)

Soils have been sampled in the vicinity of the Tomsk-Seversk facility (Siberia, Russia) that allows us to measure radioactive contaminations due to atmospheric and aquatic releases. Indeed soils exhibit large inventories of man-made fission products including 137Cs (ranging from 33,000 to 68,500 Bq m(-2)) and actinides such as plutonium (i.e. 239+240Pu from 420 to 5900 Bq m(-2)) or 241Am (160-1220 Bq m(-2)). Among all sampling sites, the bank of the Romashka channel exhibits the highest radioisotope concentrations. At this site, some short half-life gamma emitters were detected as well indicating recent aquatic discharge in the channel. In comparison, soils that underwent atmospheric depositions like peat and forest soils exhibit lower activities of actinides and 137Cs. Soil activities are too high to be related solely to global fallout and thus the source of plutonium must be discharges from the Siberian Chemical Combine (SCC) plant. This is confirmed by plutonium isotopic ratios measured by ICP-MS; the low 241Pu/239Pu and 240Pu/239Pu atomic ratios with respect to global fallout ratio or civil nuclear fuel are consistent with weapons grade signatures. Up to now, the influence of Tomsk-Seversk plutonium discharges was speculated in the Ob River and its estuary. Isotopic data from the present study show that plutonium measured in SCC probably constitutes a significant source of plutonium in the aquatic environment, together with plutonium from global fallout and other contaminated sites including Tomsk, Mayak (Russia) and Semipalatinsk (Republic of Kazakhstan). It is estimated that the proportion of plutonium from SCC source can reach 45% for 239Pu and 60% for 241Pu in the sediments.     

Determination of the origin of unknown irradiated nuclear fuel

An isotopic fingerprinting method is presented to determine the origin of unknown nuclear material with forensic importance. Spent nuclear fuel of known origin has been considered as the 'unknown' nuclear material in order to demonstrate the method and verify its prediction capabilities. The method compares, using factor analysis, the measured U, Pu isotopic compositions of the 'unknown' material with U, Pu isotopic compositions simulating well known spent fuels from a range of commercial nuclear power stations. Then, the 'unknown' fuel has the same origin as the commercial fuel with which it exhibits the highest similarity in U, Pu compositions.     

Discrimination of source reactor type by multivariate statistical analysis of uranium and plutonium isotopic concentrations in unknown irradiated nuclear fuel material

The problem of identifying the provenance of unknown nuclear material in the environment by multivariate statistical analysis of its uranium and/or plutonium isotopic composition is considered. Such material can be introduced into the environment as a result of nuclear accidents, inadvertent processing losses, illegal dumping of waste, or deliberate trafficking in nuclear materials. Various combinations of reactor type and fuel composition were analyzed using Principal Components Analysis (PCA) and Partial Least Squares Discriminant Analysis (PLSDA) of the concentrations of nine U and Pu isotopes in fuel as a function of burnup. Real-world variation in the concentrations of (234)U and (236)U in the fresh (unirradiated) fuel was incorporated. The U and Pu were also analyzed separately, with results that suggest that, even after reprocessing or environmental fractionation, Pu isotopes can be used to determine both the source reactor type and the initial fuel composition with good discrimination.     

Deposition and distribution of Chernobyl fallout fission products and actinides in a Russian soil profile

In this article the distribution of fission products and actinides in a soil profile from Novo Bobovicky in Russia, which was contaminated due to the Chernobyl nuclear power plant accident, is described. The ground deposition of long-lived fission products determined by gamma-spectrometry was (recalculated to 26 April 1986) 1600 kBq (137)Cs/m(2), 900 kBq (134)Cs/m(2) and 60 kBq (125)Sb/m(2). Of these radionuclides (137)Cs shows the dominating activity at the present time. After 6.5 years 90% of the Cs and Sb activity was contained in the upper 4 cm. A (239,240)Pu ground deposition of 77.4+/-8.0 Bq/m(2) was determined by alpha-spectrometry. The (238)Pu/(239,240)Pu activity ratio of 0.30+/-0.03 and (241)Pu/(239,240)Pu activity ratio of 115+/-14 (in 1986) measured in the soil profile, indicates that the analysed Pu originates mainly from the Chernobyl accident. The average (234)U/(238)U activity ratio of 1.06+/-0.29 indicates that the uranium in this soil is dominated by naturally occurring uranium.The alpha- and beta-autoradiography revealed that the activity is mainly present in particulate form. It could further be observed that the spots containing alpha- or beta-activity originated from different particles. A comparison of alpha-autoradiography with the bulk Pu and Am activity showed that 92% of the alpha-activity was present as clearly detectable alpha-spots.The beta-active particles, located by beta-autoradiography were correlated with gamma-spectrometric measurements and contained only (137)Cs. These hot spots ranged from 0.02 to 0.15 Bq.It could be concluded that the vertical transport of (137)Cs and fuel fragments occurs mainly by movement of particles through the soil. It could also be concluded that the fuel fragments found, in this soil were depleted in respect to Cs, Sb and Eu.Comparison of the analysed (238)Pu/(239,240)Pu, (241)Pu/(239,240)Pu and (241)Am/(239,240)Pu ratios with the ratios calculated with ORIGEN-S code gave an estimate of the average burn-up of the fuel particles to be in the range of 11-12 GWd/tU.The results presented in this article are valid for this single soil profile and should not be generalised unless validated in a more rigorous study of a larger number of soil profiles.     

Radioactivity measurements in moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis) samples collected from Marmara region of Turkey

The present study was conducted to compare the ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U activity concentrations in epigeic moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis). The activity levels in 37 moss and 38 lichen samples collected from the Marmara region of Turkey were measured using a gamma spectrometer equipped with a high purity germanium (HPGe) detector. The activity concentrations of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U in the moss samples were found to be in the range of 0.36-8.13, 17.1-181.1, 1.51-6.17, and 0.87-6.70 Bq kg⁻¹ respectively, while these values were below detection limit (BDL)-4.32, 16.6-240.0, 1.32-6.47, and BDL-3.57 Bq kg⁻¹ respectively in lichen. The average moss/lichen activity ratios of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U were found to be 1.32 ± 0.57, 2.79 ± 1.67, 2.11 ± 0.82, and 2.19 ± 1.02, respectively. Very low ¹³⁷Cs concentrations were observed in moss and lichen samples compared to soil samples collected from the same locations in a previous study. Seasonal variations of the measured radionuclide activities were also examined in the three sampling stations.     

Residual radioactive contamination at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" in the Republic of Sakha (Yakutia)

In this paper, results are reported on the concentrations and activity ratios of 137Cs, 239+240Pu and 238Pu in soils, lichen and bottom sediments collected at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" (Republic of Sakha (Yakutia), North-East Siberia). At the "Craton-3" site, 239- 240Pu concentrations in the range 6.2 mBq/g to 5.9 Bq/g in surface soils (0-5 cm) and 239+240Pu concentrations up to 7.4 Bq/g in lichen were observed. The 137Cs concentration in measured soils range from 0.52 to 216 Bq/g for the near-plume and from 1.65 to 21.5 Bq/g for the far-plume. In lichen, 137Cs concentration varied from a global background level up to 251 Bq/g. Radioactive contamination at "Crystal" demonstrates an extremely irregular distribution of 239,240Pu and 137Cs in environmental samples taken at locations within 150 m radius of the site. Further work on compiling detailed maps of radioactive contamination of the territory around "Craton-3" and "Crystal" is discussed.     

Isotopic signature of atmospheric xenon released from light water reactors

A global monitoring system for atmospheric xenon radioactivity is being established as part of the International Monitoring System to verify compliance with the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The isotopic activity ratios of (135)Xe, (133m)Xe, (133)Xe and (131m)Xe are of interest for distinguishing nuclear explosion sources from civilian releases. Simulations of light water reactor (LWR) fuel burn-up through three operational reactor power cycles are conducted to explore the possible xenon isotopic signature of nuclear reactor releases under different operational conditions. It is studied how ratio changes are related to various parameters including the neutron flux, uranium enrichment and fuel burn-up. Further, the impact of diffusion and mixing on the isotopic activity ratio variability are explored. The simulations are validated with reported reactor emissions. In addition, activity ratios are calculated for xenon isotopes released from nuclear explosions and these are compared to the reactor ratios in order to determine whether the discrimination of explosion releases from reactor effluents is possible based on isotopic activity ratios.     

Distribution of Np and Pu in Swedish lichen samples (Cladonia stellaris) contaminated by atmospheric fallout

The activity concentrations of (237)Np and the two Pu isotopes, (239)Pu and (240)Pu, were determined in lichen samples (Cladonia stellaris) contaminated by fallout from atmospheric nuclear test explosions and the Chernobyl accident. The samples were collected at 18 locations in Sweden, from north to south, between 1986 and 1988 and analysed with high-resolution inductively coupled plasma mass spectrometry (HR-ICP-MS) and alpha spectrometry. Data on the activity ratios (238)Pu/(239+240)Pu and (134)Cs/(137)Cs measured previously were also included in this study for comparison. The (237)Np activity concentration ranged from 0.08 +/- 0.01 to 2.08 +/- 0.17 MBq kg(-1), depending on the location of the sampling site and time of collection. The (239+240)Pu activity concentration ranged from 0.09 +/- 0.01 to 4.09 +/- 0.15 Bq kg(-1), with the (240)Pu/(239)Pu atomic ratio ranging between 0.16 +/- 0.01 and 0.44 +/- 0.03, the higher ratios indicating a combination of weapons test fallout and Chernobyl fallout. The (237)Np/(239)Pu atomic ratios ranged between 0.06 +/- 0.01 and 0.42 +/- 0.04, the lower ratios indicating combination of weapons test fallout and Chernobyl fallout. At a well-defined sampling site at Lake Rogen (62.32 degrees N, 12.38 degrees E), additional lichen samples were collected between 1987 and 1998 to study the distribution of Np and Pu in different layers. The concentrations of the two elements follow each other quite well in the profile.     

Distribution of uranium and radium isotopes in an aquifer of a semi-arid region (Manouba-Essijoumi, Northern Tunisia)

Groundwaters from the Sebkhet Essijoumi drainage basin, situated in northern Tunisia, West of the city of Tunis, were sampled and analyzed for uranium and radium isotopes. Low (234)U/(238)U activity ratios coupled with relatively high (228)Ra and (238)U concentrations were found in the Manouba plain phreatic aquifer, at the northern part of the basin, where remote sensing has indicated that this plain corresponds to the main humid zone of the area. Low (234)U/(238)U ratios probably reflected short residence time for waters in the Manouba plain, and high ratios longer residence time in the south, where water reaching the phreatic aquifer seems to have previously circulated in rocks constituting the southern hills. Assuming that, in the Manouba plain aquifer, the groundwater flows downstream from the Oued Lill pass area to the South-West of the Sebkha, the difference in the (228)Ra/(226)Ra activity ratio suggests that the residence time of water has been 2.8 years longer near the Sebkha than upstream.     

Intraspecific variation in the viability of soredia in <Emphasis Type="Italic">Hypogymnia physodes</Emphasis> (L.) Nyl. (Ascomycota: Lecanorales)

The contribution of morphological features of parent thalli, substrate and climatic factors, and their seasonal fluctuations to variation in the viability of vegetative diaspores has been studied on the model of epiphytic lichen Hypogymnia physodes. Seasonal trends in viability have been revealed only in certain types of biotopes. Hygrothermal conditions and substrate properties in the biotope have proved to have a significant effect on the viability of soredia.     

Revision and meta-analysis of selected biosphere parameter values for chlorine, iodine, neptunium, radium, radon and uranium

There is a continual supply of new experimental data that are relevant to the assessment of the potential impacts of nuclear fuel waste disposal. In the biosphere, the traditional assessment models are data intensive, and values are needed for several thousand parameters. This is augmented further when measures of central tendency, statistical dispersion, correlations and truncations are required for each parameter to allow probabilistic risk assessment. Recent reviews proposed values for 10-15 key element-specific parameters relevant to (36)Cl, (129)I, (222)Rn, (226)Ra, (237)Np and (238)U, and some highlights from this data update are summarized here. Several parameters for Np are revised downward by more than 10-fold, as is the fish/water concentration ratio for U. Soil solid/liquid partition coefficients, Kd, are revised downward by 10-770-fold for Ra. Specific parameters are discussed in detail, including degassing of I from soil; sorption of Cl in soil; categorization of plant/soil concentration ratios for U, Ra and Np; Rn transfer from soil to indoor air; Rn degassing from surface water; and the Ca dependence of Ra transfers.     

Quantitative assessment of the long term behaviour of 90Sr in Lake Uruskul,Southern Urals,Russia

The present paper is aimed at assessing the long term behaviour of 90Sr migration from water to bottom sediments of Lake Uruskul, Southern Urals, Russia. The lake was contaminated following the nuclear accident at the Mayak nuclear complex in 1957 (the Kyshtym accident). Some transfer parameters relevant to the behaviour of 90Sr in the water-sediment system were evaluated: a) the radionuclide migration velocity from the water column to the bottom sediment, b) the radionuclide migration rate from bottom sediment to water, and c) the radionuclide migration rate from bottom sediment to deep sediment. The estimated values of the above parameters were 6.4 x 10(-1) m s(-1), 5.7 x 10(-10) s(-1) and 5.2 x 10(-10) s(-1), respectively. These values were compared with data obtained for some Italian lakes contaminated by 90Sr after the nuclear weapons tests fallout. The relatively low radionuclide migration from water to sediment of these lakes is reflected by the values of the ratio migration velocity/migration rate from sediment to water (4 m and 12 m) that are significantly lower than the corresponding value in the Russian lake (112 m). The peculiar hydrochemical conditions of Lake Uruskul (high pH, high mineralisation, etc.) are considered to be responsible for the high radionuclide migration from water to sediment.     

三峡上游地区一次西南涡暴雨过程中尺度特征诊断和数值模拟

结合高空、地面实况观测数据以及1°×1°NCEP客观再分析资料,对2009年6月28日20时至29日20时(北京时)发生在三峡上游地区的一次区域暴雨过程进行了中尺度特征诊断,结果表明本次过程是东北低涡和副高稳定少动的大尺度环流背景形势下,由于高原低值系统在东移过程中与西南涡结合而产生的强降水天气过程。高原上不稳定能量的扰动和下传为西南涡的产生提供了必要能量条件,高低层的水汽平流和水汽辐合的交汇地带与最强降水带存在较好的一致性。另外,利用WRF中尺度数值模式对该次过程进行了数值模拟,结果显示在同化了地面和高空常规观测资料后,模式模拟效果得到明显改善,模拟降水能够大致体现该次过程的总的降水演变和分布情况,但后期模拟降水偏大。数值诊断结果发现,盆地西部与上升气流相伴的正涡度柱的演变过程与强降水的发生过程密切相关,该因子对于正确预报降水发生时间具有指示意义。     

Some observations on the geochemistry and isotopic composition of uranium in relation to the reprocessing of nuclear fuels

In order to determine whether or not uranium depleted in ²³⁵U and derived from the British Nuclear Fuels Ltd (BNFL) nuclear fuel reprocessingg plant at Sellafield, Cumbria, UK can be detected in environmental samples, we have investigated the isotopic composition of uranium in ammonium carbonate leachates from marine and terrestial samples from near Sellafield. Some show a depletion in ²³⁵U and the presence of ²³⁶U which unequivocally identifies the presence of uranium derived from BNFL. The ²³⁴U/²³⁸U activity ratio and total uranium content of samples are not significantly different from those of natural uranium abundances. The highest concentrations of uranium are found in anaerobic organic-rich silts and the lowest in sandy silts and coarse-grained sands.     

Anthropogenic 236U at Rocky Flats,Ashtabula river harbor,and Mersey estuary: three case studies by sector inductively coupled plasma mass spectrometry

236U (t(1/2)=2.3 x 10(7) y) is formed as a result of thermal neutron capture by (235)U. In naturally occurring U ores, where a high neutron flux is present from spontaneous fission of (238)U, (236)U/(238)U atom ratios are approximately 10(-4) ppm. In the natural Earth's crust, unaffected by nuclear fallout, these ratios are expected to be on the order of 10(-8) ppm. Reactor-irradiated U, however, exhibits high (236)U/(238)U atom ratios approaching 10(4) ppm. As a result, the presence of very small quantities of reactor-irradiated U will significantly enhance the "background" (236)U/(238)U atom ratio. When sufficiently elevated (236)U/(238)U ratios are present, the determination of (236)U/(238)U by rapid inductively coupled plasma mass spectrometric (ICPMS) methods is attractive. We have used sector ICPMS at medium resolving power (R=3440) to measure (236)U/(238)U atom ratios with a determination limit of 0.2 ppm. The limiting factors in the measurement are the (235)U(1)H(+) isobar and background signal at m/z 236 arising from the (238)U(+) peak tail. Based upon the analysis of replicates and considerations of possible systematic errors, uncertainties of +/-5% are found for (236)U/(238)U atom ratios of 1-100 ppm. This procedure has been demonstrated in studies of anthropogenic (236)U in the environment at three locations: (a) offsite soils from the vicinity of the Rocky Flats Environmental Technology site (Golden, Colorado, USA); (b) sediments from the Ashtabula River (Ohio, USA); and (c) sediments from the Mersey estuary (Liverpool, UK). In each of these three locations, definite plumes of elevated (236)U/(238)U are identified and characterized. Maximum (236)U/(238)U atom ratios observed in RFETS-vicinity soils, the Ashtabula River, and the Mersey Estuary are 2.8, 140, and 4.4 ppm, respectively.     

A study of radionuclides, metals and stable lead isotope ratios in sediments and soils in the vicinity of natural U-mineralisation areas in the Northern Territory

Australian guidelines recommend that tailings materials from uranium (U) mining and milling be contained without any detrimental impact on the environment for at least 1000 years. Natural analogue sites are being investigated to determine if they can provide data on the rates of natural erosion processes which occur over these timescales, for input into predictive geomorphic computer models. This paper presents radionuclide, metal and stable lead (Pb) isotope data from sediment cores and surface soils in the vicinity of two mineralised areas in the Alligator Rivers Region.Surface scrapes from the natural Anomaly #2, south of the Ranger mineral lease, exhibit radiogenic ²⁰⁶Pb/²⁰⁷Pb and ²⁰⁸Pb/²⁰⁷Pb ratios, and elevated U and metal concentrations typical for a near surface U anomaly. In contrast, samples taken from the Koongarra mineral lease (KML) show radionuclide activity and metal concentrations similar to natural areas elsewhere in the Alligator Rivers Region and Pb isotope ratios are closer to present day average crustal ratios (PDAC), as the orebodies at KML are covered by surficial sand. A sediment core collected from Anbangbang Billabong, downstream of KML, exhibits small variations in Pb isotope ratios that indicate that approximately 1% of the upper sediments in the sediment core may be derived from material originating from the U anomaly at Koongarra.     

Radium geochemistry in Na-Cl type groundwater in Niigata Prefecture, Japan

Radium isotopes in 23 Na-Cl type groundwater sampled mainly from deep wells in Niigata Prefecture, which is the site of the largest oil- and gas-fields in Japan, were measured along with U isotopes, chemical components and hydrogen and oxygen isotope ratios to elucidate the distribution and behavior of Ra in a brackish environment underground. Also analyzed were U and Th isotopes in 38 rock samples collected from outcrops at 17 locations. Ra-226 concentrations (8.86-1637 mBq kg⁻¹) of groundwater samples roughly correlated with total dissolved solid (TDS) concentrations and other alkaline earth contents. Their ²²⁸Ra/²²⁶Ra activity ratios (0.32-5.2) were similar to or higher than the ²³²Th/²³⁸U activity ratios (0.6-1.7) in the rocks. The most likely transport mechanism of Ra isotopes into groundwater was due to their α-recoil from the solid phase, probably from the water-rock interface where Th isotopes had accumulated, and adsorption/desorption reaction based on the increase in ²²⁶Ra contents with TDS.